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Mesoporous mixed oxide materials as a new class of SO2 resistant catalysts for hydrocarbon oxidation

a technology of mixed oxide materials and hydrocarbon oxidation, which is applied in the direction of catalyst activation/preparation, alkali metal oxides/hydroxides, metal/metal-hydroxide catalysts, etc., can solve the problems of low specific surface area of materials and limited potential applications as catalysts, and achieve high catalyst activity, high specific surface area, and high component dispersion

Inactive Publication Date: 2006-11-07
UNIV LAVAL
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

The present invention provides a new method for synthesizing a new type of ternary mesoporous mixed oxide materials (e.g., La—Co—Zr oxides, La—Mn—Zr oxides, La—Co—Ce oxides etc.). These materials have high surface area, are thermally robust, and have high component dispersion. Additionally, these materials exhibit unusually high catalytic activity for hydrocarbon oxidation with high resistance to SO2 poisoning. The invention also relates to the synthesis of ordered mesoporous mixed oxides of lanthanum, of a metal selected from the group consisting of Cr, Mn, Fe, Co, Ni, Cu and Zn, and of zirconium or cerium. These materials have a high surface area, a high component dispersion, and nano-crystalline channel walls after calcinating at a temperature higher than 450° C. The highly ordered mesoporous mixed oxides may contain dopants such as palladium, platinum, nickel or mixtures thereof.

Problems solved by technology

However, these materials usually possess low specific surface areas and are severely poisoned by a few ppm SO2.
Their potential applications as catalysts are therefore limited.

Method used

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  • Mesoporous mixed oxide materials as a new class of SO2 resistant catalysts for hydrocarbon oxidation
  • Mesoporous mixed oxide materials as a new class of SO2 resistant catalysts for hydrocarbon oxidation
  • Mesoporous mixed oxide materials as a new class of SO2 resistant catalysts for hydrocarbon oxidation

Examples

Experimental program
Comparison scheme
Effect test

example 1

[0047]This example concerns the preparation of mesoporous La—Co—Zr mixed oxide materials with various atomic (La+Co / La+Co+Zr) ratios (designated as Meso LCZ[x] where x=(La+Co) / La+Co+Zr). They are prepared from amorphous La—Co citrate complex precursor as La and Co source, zirconium sulfate as Zr source, and cetyltrimethylammonium bromide (CTAB) as the surfactant.

[0048]The La—Co precursor was prepared according to Baythoum and Sale (Baythoun, M. S. G. and Sale, F. R., J. Mat. Sci., 17, 1982, 2757). In a typical synthesis, for the Meso-LCZ material with x=0.5, the La—Co citratè complex precursor was prepared from 1.65 g of lanthanum nitrate, La(NO3)3.6H2O, 1.45 g of cobalt nitrate, Co(NO3)2.6H2O (atomic Co / La=1), and 1.92 g of citric acid. 7.0 g of CTAB was dissolved in 120 g of distilled water and 30 g of HCl 10%. Then, the La—Co citrate complex precursor and 3.55 g of zirconium sulfate dissolved in 100 g of distilled water were added, giving a clear homogeneous solution.

[0049]The mi...

example 2

[0053]Preparation of mesoporous La—Mn—Zr mixed oxide materials with an atomic (La+Mn / La+Mn+Zr) ratio of 0.5 (designated as Meso LMZ[0.5]). The synthesis was performed operating under the conditions described in example 1, except that manganese nitrate was used instead of cobalt nitrate for the preparation of an amorphous La—Mn citrate complex precursor. FIG. 6 shows the N2 adsorption / desorption isotherms of the Meso LMZ[0.5] sample after calcination at 400° C. for 8 h. It exhibits the typical behaviour of mesoporous molecular sieves. The specific surface area and pore volume were 205 m2 / g and 0.115 cm3 / g, respectively. The inset in FIG. 6 shows the BJH pore size distribution. The narrow pore size distribution with a pore diameter of about 22.5 Å indicates the textural uniformity of the materials. Table 2 also summarizes the physico-chemical properties of the Meso LMZ[0.5] sample after calcination for 8 h at different temperatures. The pore size diameters are substantially enlarged w...

example 3

[0054]This example illustrates the preparation of mesoporous La—Co—Zr mixed oxide materials with an atomic (La+Co / La+Co+Zr) ratio of 0.5 (namely Meso LCZ[0.5]) using metal acetate precursor as Co and La sources. The synthesis was also performed operating under the conditions described in example 1 except that cobalt acetate and lanthanum acetate were used instead of amorphous La—Co citrate complex precursor and no citric acid was added. The Meso LCZ[0.5] sample was also calcined in air at different temperatures (e.g. 400, 500 and 600° C.) for 8 h. The N2 adsorption / desorption isotherms of these samples were also carried out and the results are summarized in Table 3. Similar trends were observed for this Meso LCZ[0.5] sample as compared to the Meso LMZ[0.5] sample after calcination at different temperatures.

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Abstract

The oxide materials are of the class of ternary mesoporous mixed oxide materials including lanthanum, a metal M selected from the group consisting of Cr, Mn, Fe, Co, Ni, Cu and Zn, and zirconium or cerium such a mesoporous La—Co—Zr mixed oxide material designated as Meso LCZ[x] where x is the atomic ratio (La+Co) / La+Co+Zr. They are useful as catalysts since they show high activities for hydrocarbon oxidation and good resistance against poisoning agents. These highly ordered mesoporous mixed oxides are synthesized by: preparing an amorphous solution of a La-M precursor and adding a salt of zirconium or cerium thereto; acidifying the amorphous solution in the presence of a surfactant under conditions to obtain a clear homogeneous solution; adjusting pH of the solution under conditions to form a solid precipitate; separating the solution and surfactant from the precipitate; and calcinating the precipitate.

Description

BACKGROUND OF THE INVENTION[0001]1. Field of the Invention[0002]The present invention relates to mesoporous mixed oxide materials as a new class of SO2 resistant catalysts for hydrocarbon oxidation and a method for preparing the same. The mesoporous mixed oxide of this invention are ternary materials comprising lanthanum, a metal M selected from the group consisting of Cr, Mn, Fe, Co, Ni, Cu and Zn, and zirconium or cerium.[0003]2. Description of Prior Art[0004]The significant advantages of catalytic combustion of hydrocarbons include the more efficient use of energy source and minimum pollutant emissions as compared to convention flame combustion. Catalytic combustion at low temperature plays therefore an important role in energy supply for industrial and domestic applications. In the case of methane oxidation, the light-off point (defined as 10% conversion of the fuel stream) should ideally be achieved at a temperature of about 400° C. Therefore, in this context, catalytic materia...

Claims

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Application Information

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Patent Type & Authority Patents(United States)
IPC IPC(8): C01F1/00B01J23/10C01F17/00B01J23/83B01J29/03B01J35/10B01J37/03C01B37/00C01G45/00C01G51/00
CPCB01J23/002B01J23/83B01J29/0308B01J35/1061B01J37/036C01B37/00C01G45/006C01G51/006C01G51/70C01G49/009C01G53/006B01J2523/00C01P2002/34C01P2002/52C01P2002/72C01P2002/74C01P2004/04C01P2006/12C01P2006/14C01P2006/16C01P2006/17C01P2006/40B01J2523/3706B01J2523/48B01J2523/72B01J2523/845C01P2004/03C01P2004/62B01J35/647
Inventor KALIAGUINE, SERGEDO, TRONG ON
Owner UNIV LAVAL
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